{"title":"Fe、Ga和Mo改性ZnCu-MOF和ZnCuAl-LDH复合催化剂催化CO2加氢制甲醇","authors":"Ziyuan Li, Mingsheng Luo, Zhi Yang, Xiaoteng Cui, Wenshuai Yang, Lingman Xia, Changke Shao, Roshni Rahman","doi":"10.1007/s10562-024-04910-9","DOIUrl":null,"url":null,"abstract":"<div><p>To effectively mitigate the global warming issue, it is crucial to develop advanced technologies that can significantly reduce carbon dioxide emissions. CO<sub>2</sub> hydrogenation for methanol synthesis is increasingly recognized as a promising chemical approach for the green-house gas utilization. In this study, we present a highly active, selective and stable Mo modified ZnCu-MOF and ZnCuAl-LDH composite catalysts, which achieves 18% CO<sub>2</sub> conversion and 70% methanol selectivity at 230 °C, 3.0 MPa at a space velocity of 3600 mL·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>. Furthermore, after 140 h of operation, the catalyst demonstrates superior durability. In-situ DRIFT results reveal that this CO<sub>2</sub> hydrogenation reaction over the ZnCu-MOF and ZnCuAl-LDH composite catalysts proceeds through key intermediate formate species, ultimately leading to the methanol formation. In contrast, the Mo-modified catalysts facilitate the CO insertion reaction (CO<sub>2</sub> → CO*, CO* + *CH<sub>x</sub> → CH<sub>3</sub>OH), thereby enhancing the methanol yield.</p><h3>Graphical Abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 2","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CO2 Hydrogenation to Produce Methanol over Fe, Ga and Mo Modified ZnCu-MOF and ZnCuAl-LDH Composite Catalysts\",\"authors\":\"Ziyuan Li, Mingsheng Luo, Zhi Yang, Xiaoteng Cui, Wenshuai Yang, Lingman Xia, Changke Shao, Roshni Rahman\",\"doi\":\"10.1007/s10562-024-04910-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>To effectively mitigate the global warming issue, it is crucial to develop advanced technologies that can significantly reduce carbon dioxide emissions. CO<sub>2</sub> hydrogenation for methanol synthesis is increasingly recognized as a promising chemical approach for the green-house gas utilization. In this study, we present a highly active, selective and stable Mo modified ZnCu-MOF and ZnCuAl-LDH composite catalysts, which achieves 18% CO<sub>2</sub> conversion and 70% methanol selectivity at 230 °C, 3.0 MPa at a space velocity of 3600 mL·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>. Furthermore, after 140 h of operation, the catalyst demonstrates superior durability. In-situ DRIFT results reveal that this CO<sub>2</sub> hydrogenation reaction over the ZnCu-MOF and ZnCuAl-LDH composite catalysts proceeds through key intermediate formate species, ultimately leading to the methanol formation. In contrast, the Mo-modified catalysts facilitate the CO insertion reaction (CO<sub>2</sub> → CO*, CO* + *CH<sub>x</sub> → CH<sub>3</sub>OH), thereby enhancing the methanol yield.</p><h3>Graphical Abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 2\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-01-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-024-04910-9\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-024-04910-9","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
CO2 Hydrogenation to Produce Methanol over Fe, Ga and Mo Modified ZnCu-MOF and ZnCuAl-LDH Composite Catalysts
To effectively mitigate the global warming issue, it is crucial to develop advanced technologies that can significantly reduce carbon dioxide emissions. CO2 hydrogenation for methanol synthesis is increasingly recognized as a promising chemical approach for the green-house gas utilization. In this study, we present a highly active, selective and stable Mo modified ZnCu-MOF and ZnCuAl-LDH composite catalysts, which achieves 18% CO2 conversion and 70% methanol selectivity at 230 °C, 3.0 MPa at a space velocity of 3600 mL·gcat−1·h−1. Furthermore, after 140 h of operation, the catalyst demonstrates superior durability. In-situ DRIFT results reveal that this CO2 hydrogenation reaction over the ZnCu-MOF and ZnCuAl-LDH composite catalysts proceeds through key intermediate formate species, ultimately leading to the methanol formation. In contrast, the Mo-modified catalysts facilitate the CO insertion reaction (CO2 → CO*, CO* + *CHx → CH3OH), thereby enhancing the methanol yield.
期刊介绍：
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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